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Fast-ion conduction and local environments in BIMEVOX.

Harry J Stroud1, Chris E Mohn2, Jean-Alexis Hernandez2

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Density functional theory reveals the complex energy landscape of bismuth vanadate (Bi4V2O11), a fast-ion conductor. Oxygen ion diffusion primarily occurs within vanadium layers, aligning with experimental findings.

Keywords:
BIMEVOXab initioconduction mechanismdisorderionic conductivitymolecular dynamics

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Area of Science:

  • Solid-state chemistry
  • Materials science
  • Computational materials science

Background:

  • Fast-ion conductors are crucial for energy storage and conversion technologies.
  • Bismuth vanadate (Bi4V2O11) is a promising material for solid oxide fuel cells due to its high ionic conductivity.
  • Understanding the atomistic mechanisms governing ion transport is key to optimizing material performance.

Purpose of the Study:

  • To investigate the energy landscape and ion diffusion mechanisms in Bi4V2O11 using first-principles calculations.
  • To elucidate the role of oxygen vacancies and their distribution in facilitating ionic conductivity.
  • To compare ion conduction pathways in Bi4V2O11 with those in related materials like Bi2O3.

Main Methods:

  • Density functional theory (DFT) was employed to map the energy landscape and identify low-energy configurations.
  • Ab initio molecular dynamics (AIMD) simulations were used to study oxygen ion diffusion pathways at finite temperatures.
  • Calculated ionic conductivity was compared with experimental data.

Main Results:

  • A high density of low-energy minima was found, characterized by uniform oxygen vacancy distribution across vanadium-oxygen layers.
  • Oxygen ion diffusion predominantly occurs within the vanadium-oxygen layers along the <110> directions, involving O(2) and O(3) sites.
  • Oxygen vacancies in Bi-O layers are replenished by oxygen migration from V-O layers, and calculated ionic conductivity shows good agreement with experimental values.

Conclusions:

  • The study clarifies the dominant diffusion pathways in Bi4V2O11, highlighting the importance of cooperative ion motion within vanadium-oxygen layers.
  • The findings provide insights into the factors controlling ionic conductivity in this fast-ion conductor.
  • The comparison with Bi2O3 contributes to a broader understanding of ion conduction in related oxide materials.